Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent material...Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.展开更多
Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance i...Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.展开更多
Although supported solid amine adsorbents have attracted great attention for CO_(2) capture,critical chemical deactivation problems including oxidative degradation and urea formation have severely restricted their pra...Although supported solid amine adsorbents have attracted great attention for CO_(2) capture,critical chemical deactivation problems including oxidative degradation and urea formation have severely restricted their practical applications for flue gas CO_(2) capture.In this work,we reveal that the nature of surface hydroxyl groups(metal hydroxyl Al–OH and nonmetal hydroxyl Si–OH)plays a key role in the deactivation mechanisms.The polyethyleneimine(PEI)supported on Al–OH-containing substrates suffers from severe oxidative degradation during the CO_(2) capture step due to the breakage of amine-support hydrogen bonding networks,but exhibits an excellent anti-urea formation feature by preventing dehydration of carbamate products under a pure CO_(2) regeneration atmosphere.In contrast,PEI supported on Si–OHcontaining substrates exhibits excellent anti-oxidative stability under simulated flue gas conditions by forming a robust hydrogen bonding protective network with Si–OH,but suffers from obvious urea formation during the pure CO_(2) regeneration step.We also reveal that the urea formation problem for PEI-SBA-15 can be avoided by the incorporation of an OH-containing PEG additive.Based on the intrinsic understanding of degradation mechanisms,we successfully synthesized an adsorbent 40PEI-20PEG-SBA-15 that demonstrates outstanding stability and retention of a high CO_(2) capacity of 2.45 mmol g^(−1) over 1000 adsorption–desorption cycles,together with negligible capacity loss during aging in simulated flue gas(10%CO_(2)+5%O_(2)+3%H_(2)O)for one month at 60–70℃.We believe this work makes great contribution to the advancement in the field of ultra-stable solid amine-based CO_(2) capture materials.展开更多
A series of copper-based activated carbon (AC) adsorbents were prepared in order to investigate the effect of Zn, Ce addition on Cu-based AC adsorbent for phosphine (PH3) adsorption removal from yellow phosphorous tai...A series of copper-based activated carbon (AC) adsorbents were prepared in order to investigate the effect of Zn, Ce addition on Cu-based AC adsorbent for phosphine (PH3) adsorption removal from yellow phosphorous tail gas. N2 adsorption isotherm and X-ray diffrac-tion (XRD) results suggested that the addition of Zn could increase the adsorbent ultramicropores, decrease the adsorbent supermicropores and the adsorbent average pore diameter. Therefore it enhanced the PH3 adsorption capacity. Appropriate amoun...展开更多
The increase in energy demand caused by industrialization leads to abundant CO_2 emissions into atmosphere and induces abrupt rise in earth temperature. It is vital to acquire relatively simple and cost-effective tech...The increase in energy demand caused by industrialization leads to abundant CO_2 emissions into atmosphere and induces abrupt rise in earth temperature. It is vital to acquire relatively simple and cost-effective technologies to separate CO_2 from the flue gas and reduce its environmental impact. Solid adsorption is now considered an economic and least interfering way to capture CO_2, in that it can accomplish the goal of small energy penalty and few modifications to power plants. In this regard, we attempt to review the CO_2 adsorption performances of several types of solid adsorbents, including zeolites, clays, activated carbons, alkali metal oxides and carbonates, silica materials, metal–organic frameworks, covalent organic frameworks, and polymerized high internal phase emulsions. These solid adsorbents have been assessed in their CO_2 adsorption capacities along with other important parameters including adsorption kinetics, effect of water, recycling stability and regenerability. In particular,the superior properties of adsorbents enhanced by impregnating or grafting amine groups have been discussed for developing applicable candidates for industrial CO_2 capture.展开更多
Two organobentonites were synthesized by placing quaternary ammonium cationscetyltrimethylammonium bromide (CTMAB) and cetylpyridinium chloride (CPC) on bentonite bycation exchange. Their ability to adsorb phenol, ani...Two organobentonites were synthesized by placing quaternary ammonium cationscetyltrimethylammonium bromide (CTMAB) and cetylpyridinium chloride (CPC) on bentonite bycation exchange. Their ability to adsorb phenol, aniline. nitrobenzene and p-nitrophenol were examined.The optimal conditions for organobentonites to remove the organic pollutants from waterwere studied. The removal rates for organobentonites to treat the organic compounds in water werefound to be over 8 times for the original mineral (untreated bentonite).The removal rates of organic pollutants and COD of wastewater were further improved by organobentonites in the presence of aluminum sulfate. The structure of organobentonites and the mechanism for their adsorption were investigated by X-ray diffraction (XRD) analysis, infrared spectra and BET surface area.展开更多
Phosphine(PH3) is a highly toxic air pollutant,commonly produced in phosphorous chemical industry.But it has received less research attention due to its handling difficultly.CO is the main content of the phosphorous c...Phosphine(PH3) is a highly toxic air pollutant,commonly produced in phosphorous chemical industry.But it has received less research attention due to its handling difficultly.CO is the main content of the phosphorous chemical industry tail gas,the concentration of which is always more than 80 vol.%,and it can be the feed gas to produce various valuable products such as formate,oxalate,and methanol and so on.But,PH3 is one of the important barriers,which is harmful to the following chemical process.In order to make use of the tail gas,PH3 should be removed firstly,and CO should be covered in the whole purified procedure at the same time.In this work,the modified activated carbon(MAC) was used as the adsorbent to separate PH3 from the mixture tail gas.Series of MAC adsorbents were prepared for the adsorption of PH3,which loaded Cu-Fe and Ce(La),or separately.The PH3 adsorption capacities,chemical and physical properties of MAC were all investigated.The results showed that over 99% PH3 adsorption efficiency was achieved when used MAC adsorbents.The removal efficiency and PH3 adsorption capacity of the Cu-Fe-Ce/AC(20:1:0.4) were both much higher than those modified activated carbons.The maximum PH3 adsorption capacity was 71 mg of PH3/g of MAC on the Cu-Fe-Ce/AC,which were much higher than literature data using CuO only for adsorbing hydride gases.展开更多
In this study, we prepared and applied polymeric porous microsphere adsorbents with selectivity for Li^+ extraction from aqueous solution. We synthesized the adsorbents by suspension polymerization using methacryloyox...In this study, we prepared and applied polymeric porous microsphere adsorbents with selectivity for Li^+ extraction from aqueous solution. We synthesized the adsorbents by suspension polymerization using methacryloyoxyme-12-crown-4(M12C4) as a functional monomer, which had been synthesized from 2-hyroxymethyl-12-crown-4 and methacryloyl chloride. We verified the chemical composition by solid nuclear magnetic resonance(13C-NMR) spectroscopy and observed the porous structure by scanning electron microscopy(SEM). We conducted adsorption isothermal and kinetic tests to determine the adsorption properties. It was found that the adsorbents showed high adsorption efficiency and an adsorption equilibrium time of 200 min. In addition, since the crown ether used in this work could form a stable complex with Li^+, we observed good selectivity for Li^+ in the prepared solution compared with other ions such as Na^+, K^+, Mg^(2+), and Ca^(2+). We reused the adsorbents five times with no significant decrease in adsorptive capacity.展开更多
The adsorption behavior ofp-aminobenzoic acid and o-aminobenzoic acid onto the different polymeric adsorbents was systematically investigated as a function of the solution concentration and temperature. Experimental r...The adsorption behavior ofp-aminobenzoic acid and o-aminobenzoic acid onto the different polymeric adsorbents was systematically investigated as a function of the solution concentration and temperature. Experimental results indicated that the equilibrium adsorption data of the four polymeric adsorbents fitted well in the Freundlich isotherm. The adsorption capacity of multi-functional polymeric adsorbent NJ-99 was the highest, which might be attributed to the strong hydrogen-bonding interaction between the amino groups on the resin and the carboxyl group of aminobenzoic acid. The adsorption capacity of o-aminobenzoic acid onto any adsorbent was higher than p-aminobenzoic acid. Thermodynamic studies suggested the exothermic, spontaneous physical adsorption process. Adsorption kinetics results showed that the adsorption followed the pseudo-second-order kinetics model and the intraparticle mass transfer process was the rate-controlling step.展开更多
Adsorption equilibrium isotherms of phenolic compounds, phenol, p cresol, p chlorophenol and p nitrophenol, from aqueous solutions by Amberlite XAD 4 polymeric adsorbent and its acetylized derivative M...Adsorption equilibrium isotherms of phenolic compounds, phenol, p cresol, p chlorophenol and p nitrophenol, from aqueous solutions by Amberlite XAD 4 polymeric adsorbent and its acetylized derivative MX 4 within temperature range of 283 323K were obtained and fitted to the Freundlich isotherms. The capacities of equilibrium adsorption for all four phenolic compounds from their aqueous solutions increased around 20% on the acetylized resin, which may be contributed to the specific surface area and the partial polarity on the network. Estimations of the isosteric enthalpy, free energy, and entropy for the adsorption process were reported.展开更多
This paper presents experimental observations on the adsorption of individual solutes by a simple thermodynamic framework, and the equilibrium adsorption of ethyl benzoate and diethyl phthalate on phenolic resin adsor...This paper presents experimental observations on the adsorption of individual solutes by a simple thermodynamic framework, and the equilibrium adsorption of ethyl benzoate and diethyl phthalate on phenolic resin adsorbent in hexane solutions within the temperature range of 293-313 K. The experimental results show that the Freundlich adsorption law is applicable to the adsorption of ethyl benzoate and diethyl phthalate on the adsorbent, since all the correlative factors R' are larger than 0.99. The negative values of all the isosteric adsorption enthalpies for ethyl benzoate and diethyl phthalate indicate that they undergo exothermic processes, while their magnitudes (19-28 kJ/mol) manifest a hydrogen bonding sorption process. Other thermodynamic properties: the free energy changes and the entropy change associated with the adsorption have been calculated from the Gibbs adsorption equation and the Gibbs-Helmholtz equation展开更多
Two hypercrosslinked polymeric adsorbents （ZH-01 and Amberlite XAD-4 resin） were employed to remove three kinds of phenolic compounds including phenol, 4-nitrophenol and 2,4-dinitrophenol from aqueous solutions. The...Two hypercrosslinked polymeric adsorbents （ZH-01 and Amberlite XAD-4 resin） were employed to remove three kinds of phenolic compounds including phenol, 4-nitrophenol and 2,4-dinitrophenol from aqueous solutions. The study was focused on the static equilibrium adsorption behavior, the column dynamic adsorption and desorption profiles. The Freundlich model gave a perfect fitting to the isotherm data. The adsorbing capacities for these three compounds on ZH-01 were higher than those on Amberlite XAD-4 within the temperature range 288-318 K, which was attributed to the large micropore area and 2-carboxybenzoyl functional groups on the network of ZH-01 resin. The adsorption for phenol and 4- nitrophenol on ZH-01 was a physical adsorption process, while for 2,4-dinitrophenol it was a coexistence process of physical adsorption and chemisorption＇s transitions. The column test showed the advantages of ZH-01 in the dynamic adsorption processes of phenolic compounds. Being used as the desorption reagent, sodium hydroxide solution showed an excellent performance.展开更多
The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the che...The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the chemical prelithiation agent is difficult to dope active Li^(+) in silicon-based anodes because of their low working voltage and sluggish Li^(+) diffusion rate. By selecting the lithium–arene complex reagent with 4-methylbiphenyl as an anion ligand and 2-methyltetrahydrofuran as a solvent, the as-prepared micro-sized Si O/C anode can achieve an ICE of nearly 100%. Interestingly, the best prelithium efficiency does not correspond to the lowest redox half-potential(E_(1/2)), and the prelithiation efficiency is determined by the specific influencing factors(E_(1/2), Li^(+) concentration, desolvation energy, and ion diffusion path). In addition, molecular dynamics simulations demonstrate that the ideal prelithiation efficiency can be achieved by choosing appropriate anion ligand and solvent to regulate the solvation structure of Li^(+). Furthermore, the positive effect of prelithiation on cycle performance has been verified by using an in-situ electrochemical dilatometry and solid electrolyte interphase film characterizations.展开更多
The adsorption behaviors of 1-naphthol, 1-naphthylamine and l-naphthol/l-naphthylamine mixtures in water over two macroreticular adsorbents were investigated in single or binary batch systems at 293 K, 303 K and 313 K...The adsorption behaviors of 1-naphthol, 1-naphthylamine and l-naphthol/l-naphthylamine mixtures in water over two macroreticular adsorbents were investigated in single or binary batch systems at 293 K, 303 K and 313 K respectively. All the adsorption isotherms in the studied systems can be adequately fitted by Langmuir model. In the case of aminated macroreticular adsorbent NDA103, 1-naphthol is adsorbed to a larger extent than 1-naphthylamine; while, the opposite trend is found for nonpolar macroreticular adsorbent NDA100. It is noteworthy that at higher temperature（303 K and 313 K）, the total uptake amounts of 1-naphthol and 1-naphthylamine in all binary-component systems are obvious larger than the pure uptake amounts in single-component systems, which is presumably due to the cooperative effect primarily arisen from the hydrogen-bonding interaction between the loaded 1-naphthol and 1-naphthylamine molecules. The simultaneous adsorption systems were confirmed to be helpful to the selective adsorption towards 1-naphthol according to the larger selective index.展开更多
In this article, in vitro adsorption of aflatoxin B1 （AFB1） onto different adsorbents was characterized and the result was verified by comparing the growth performance and serum protein levels of broilers exposed to...In this article, in vitro adsorption of aflatoxin B1 （AFB1） onto different adsorbents was characterized and the result was verified by comparing the growth performance and serum protein levels of broilers exposed to aflatoxin-contamination feed. Main components of adsorbents selected were yeast cell extracts （Product A）, HSCAS （Product B）, and a mixture of yeast product and HSCAS （Product C）, respectively. A total of 240 broilers were assigned to eight treatments, and the effects of three types of adsorbents on growth performance and serum protein levels were evaluated. Results indicated that Product B had the highest in vitro affinity for AFB1, followed by Product C and Product A. Product B bound 97.69% of the AFB1 in solution in 10 min, and it remained over 96.03% in 60 min at pH 8.0. The B-AFB1 complex was much stronger than the other two complexes in vitro condition （P 〈 0.05）. Feed intake （FI） and average daily gain （ADG） decreased （P 〈 0.05） and feed gain ratio increased （P 〈0.05） in the treatment fed aflatoxin-contaminated feed versus treatment on the basal feed. Serum total protein （TP）, albumin （ALB）, and globulin （GLOB） levels were significantly decreased （P〈0.05）. Product B （0.15%） increased growth performance and improved serum protein levels, Product A and Product C were not as effective as Product B. Three adsorbents tested here had sufficient potential to AFBt in some extents and Product B could bind AFB1 more effectively than Product A and Product C. These results indicated that Product B could alleviate some of the AFBt toxic effect in broilers.展开更多
The carbonaceous adsorbent was prepared from mixtures of dewatered sludge and sawdust with enhanced ZnCl2 chemical activation.Characteristics of the adsorbent were studied using scanning electron microscope(SEM) ,Four...The carbonaceous adsorbent was prepared from mixtures of dewatered sludge and sawdust with enhanced ZnCl2 chemical activation.Characteristics of the adsorbent were studied using scanning electron microscope(SEM) ,Fourier transform infrared spectroscopy(FT-IR) ,and adsorption of nitrogen.The surface analysis showed that the carbonaceous adsorbent had good specific surface and porosity(394 m 2 ·g-1of BET surface,0.12 and 0.10 ml·g-1of microporous and mesoporous volume,respectively) .The oxygen functional groups such as OH,C O and C O were found on the surface by FTIR and XPS(X-ray photoelectron spectroscopy) .The adsorption of elemental mercury(Hg0) on the carbonaceous adsorbent was studied in a fixed bed reactor.The dynamic adsorption capacity of carbonaceous adsorbent increased with influent mercury concentration,from 23.6μg·g-1at 12.58μg·m-3to 87.9μg·g-1at 72.50μg·m-3,and decreased as the adsorption temperature increased,from 246 μg·g-1 at 25°C to 61.3μg·g-1 at 140°C,when dry nitrogen was used as the carrier gas.The carbonaceous adsorbent presented higher dynamic adsorption capacity than activated carbon,which was 81.2μg·g-1and 53.8μg·g-1respectively.The adsorption data were fitted to the Langmuir adsorption model.The physical and chemical adsorption were identified on the adsorbent.展开更多
Global warming and associated global climate change have led to serious efforts towards reducing CO_(2)emissions through the CO_(2)capture from the major emission sources.CO_(2)capture using the amine functionalized a...Global warming and associated global climate change have led to serious efforts towards reducing CO_(2)emissions through the CO_(2)capture from the major emission sources.CO_(2)capture using the amine functionalized adsorbents is regard as a direct and effective way to reducing CO_(2)emissions due to their large CO_(2)adsorption amount,excellent CO_(2)adsorption selectivity and lower energy requirements for adsorbent regeneration.Moreover,large number of achievements on the amine functionalized solid adsorbent have been recorded for the enhanced CO_(2)capture in the past few years.In view of this,we review and analyze the recent advances in amine functionalized solid adsorbents prepared with different supporting materials including mesoporous silica,zeolite,porous carbon materials,metal organic frameworks(MOF)and other composite porous materials.In addition,amine functionalized solid adsorbents derived from waste resources are also reviewed because of the large number demand for cost-effective carbon dioxide adsorbents and the processing needs of waste resources.Considering the importance of the stability of the adsorbent in practical applications,advanced research in the capture cycle stability has also been summarized and analyzed.Finally,we summarize the review and offer the recommendations for the development of amine-based solid adsorbents for carbon dioxide capture.展开更多
An ultra-wideband mixing component cascaded by a mixing multi-function chip and a frequency multiplier multi-function chip was demonstrated and implemented using 3D heterogeneous integration based on the silicon adapt...An ultra-wideband mixing component cascaded by a mixing multi-function chip and a frequency multiplier multi-function chip was demonstrated and implemented using 3D heterogeneous integration based on the silicon adapter board technology.Four layers of high-resistance silicon substrate stack packaging are implemented based on the wafer-level gold-gold bonding process.Each layer adopts though silicon via(TSV)technology to realize signal interconnection.A core monolithic integrated microwave chip(MMIC)is embedded in the silicon cavity,and the silicon-based filter is integrated with the high-resistance silicon substrate.The interconnect line,cavity and filter of the silicon-based adapter board are designed with AutoCAD,and HFSS is adopted for 3D electromagnetic field simulation.According to the measured results,the radio frequency(RF)of the mixing multi-function chip is 40-44 GHz and its intermediate frequency(IF)can cover the Ku band with a chip size of 10 mm×11 mm×1 mm.The multiplier multi-function chip operates at 16-20 GHz.The fundamental suppression is greater than 50 dB and the second harmonic suppression is better than 40 dB with a chip size of 8 mm×8 mm×1 mm.The cascaded fully assembled mixing component achieves a spur of better than-50 dBc and a gain of better than 15 dB.展开更多
Hybrid adsorbents for COcapture were prepared by coassembling laponite（LP） nanosheets and 1-nbutyl-3-methylimidazolium chloride（BMIMCl）. The prepared BMIMCl/LP layered hybrids were systematically characterized. Th...Hybrid adsorbents for COcapture were prepared by coassembling laponite（LP） nanosheets and 1-nbutyl-3-methylimidazolium chloride（BMIMCl）. The prepared BMIMCl/LP layered hybrids were systematically characterized. The interlayer distance of the BMIMCl/LP layered hybrids expanded with an increasing concentration of BMIMCl, indicating that cumulative BMIMCl was intercalated into the LP layers. The efficiency of BMIMCl toward COcapture was significantly enhanced after it was immobilized within LP layers.展开更多
基金supported by Shanxi Provincial Key Research and Development Project(202102090301026)Graduate Education Innovation Project of Taiyuan University of Science and Technology(SY2023024)。
文摘Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.
基金supported by Multi-Year Research Grants from the University of Macao(MYRG-GRG2023-00010-IAPME,MYRG-GRG2024-00038-IAPME,MYRG2022-00026-IAPME)the Science and Technology Development Fund(FDCT)from Macao SAR(0023/2023/AFJ,0050/2023/RIB2,006/2022/ALC,0087/2024/AFJ,0111/2022/A2).
文摘Photoelectrochemical(PEC)water splitting holds significant promise for sustainable energy harvesting that enables efficient conversion of solar energy into green hydrogen.Nevertheless,achievement of high performance is often limited by charge carrier recombination,resulting in unsatisfactory saturation current densities.To address this challenge,we present a novel strategy for achieving ultrahigh current density by incorporating a bridge layer between the Si substrate and the NiOOH cocatalyst in this paper.The optimal photoanode(TCO/n-p-Si/TCO/Ni)shows a remarkably low onset potential of 0.92 V vs.a reversible hydrogen electrode and a high saturation current density of 39.6 mA·cm^(-2),which is about 92.7%of the theoretical maximum(42.7 mA·cm^(-2)).In addition,the photoanode demonstrates stable operation for 60 h.Our systematic characterizations and calculations demonstrate that the bridge layer facilitates charge transfer,enhances catalytic performance,and provides corrosion protection to the underlying substrate.Notably,the integration of this photoanode into a PEC device for overall water splitting leads to a reduction of the onset potential.These findings provide a viable pathway for fabricating highperformance industrial photoelectrodes by integrating a substrate and a cocatalyst via a transparent and conductive bridge layer.
基金supported by the Fundamental Research Funds for the National Natural Science Foundation of China 52225003,22208021,22109004the National Key R&D Program of China 2022YFB4101702.
文摘Although supported solid amine adsorbents have attracted great attention for CO_(2) capture,critical chemical deactivation problems including oxidative degradation and urea formation have severely restricted their practical applications for flue gas CO_(2) capture.In this work,we reveal that the nature of surface hydroxyl groups(metal hydroxyl Al–OH and nonmetal hydroxyl Si–OH)plays a key role in the deactivation mechanisms.The polyethyleneimine(PEI)supported on Al–OH-containing substrates suffers from severe oxidative degradation during the CO_(2) capture step due to the breakage of amine-support hydrogen bonding networks,but exhibits an excellent anti-urea formation feature by preventing dehydration of carbamate products under a pure CO_(2) regeneration atmosphere.In contrast,PEI supported on Si–OHcontaining substrates exhibits excellent anti-oxidative stability under simulated flue gas conditions by forming a robust hydrogen bonding protective network with Si–OH,but suffers from obvious urea formation during the pure CO_(2) regeneration step.We also reveal that the urea formation problem for PEI-SBA-15 can be avoided by the incorporation of an OH-containing PEG additive.Based on the intrinsic understanding of degradation mechanisms,we successfully synthesized an adsorbent 40PEI-20PEG-SBA-15 that demonstrates outstanding stability and retention of a high CO_(2) capacity of 2.45 mmol g^(−1) over 1000 adsorption–desorption cycles,together with negligible capacity loss during aging in simulated flue gas(10%CO_(2)+5%O_(2)+3%H_(2)O)for one month at 60–70℃.We believe this work makes great contribution to the advancement in the field of ultra-stable solid amine-based CO_(2) capture materials.
基金Project supported by the Key Program of National High Technology Research and Development Program of China (863 Program) (2008AA062602)the Young and Middle-aged Academic and Technical Back-up Personnel Program of Yunnan Province (2007PY01-10)the Analysis and Measurement Foundation of Kunming University of Science & Technology
文摘A series of copper-based activated carbon (AC) adsorbents were prepared in order to investigate the effect of Zn, Ce addition on Cu-based AC adsorbent for phosphine (PH3) adsorption removal from yellow phosphorous tail gas. N2 adsorption isotherm and X-ray diffrac-tion (XRD) results suggested that the addition of Zn could increase the adsorbent ultramicropores, decrease the adsorbent supermicropores and the adsorbent average pore diameter. Therefore it enhanced the PH3 adsorption capacity. Appropriate amoun...
基金Supported by the National Key Research & Development Program of China(2017YFB0603302)
文摘The increase in energy demand caused by industrialization leads to abundant CO_2 emissions into atmosphere and induces abrupt rise in earth temperature. It is vital to acquire relatively simple and cost-effective technologies to separate CO_2 from the flue gas and reduce its environmental impact. Solid adsorption is now considered an economic and least interfering way to capture CO_2, in that it can accomplish the goal of small energy penalty and few modifications to power plants. In this regard, we attempt to review the CO_2 adsorption performances of several types of solid adsorbents, including zeolites, clays, activated carbons, alkali metal oxides and carbonates, silica materials, metal–organic frameworks, covalent organic frameworks, and polymerized high internal phase emulsions. These solid adsorbents have been assessed in their CO_2 adsorption capacities along with other important parameters including adsorption kinetics, effect of water, recycling stability and regenerability. In particular,the superior properties of adsorbents enhanced by impregnating or grafting amine groups have been discussed for developing applicable candidates for industrial CO_2 capture.
文摘Two organobentonites were synthesized by placing quaternary ammonium cationscetyltrimethylammonium bromide (CTMAB) and cetylpyridinium chloride (CPC) on bentonite bycation exchange. Their ability to adsorb phenol, aniline. nitrobenzene and p-nitrophenol were examined.The optimal conditions for organobentonites to remove the organic pollutants from waterwere studied. The removal rates for organobentonites to treat the organic compounds in water werefound to be over 8 times for the original mineral (untreated bentonite).The removal rates of organic pollutants and COD of wastewater were further improved by organobentonites in the presence of aluminum sulfate. The structure of organobentonites and the mechanism for their adsorption were investigated by X-ray diffraction (XRD) analysis, infrared spectra and BET surface area.
基金Project supported by the Key Program of National High Technology Research and Development Program of China (863 Program) (2008AA062602)the Young and Middle-aged Academic and Technical Back-up Personnel Program of Yunnan Province (2007PY01-10)
文摘Phosphine(PH3) is a highly toxic air pollutant,commonly produced in phosphorous chemical industry.But it has received less research attention due to its handling difficultly.CO is the main content of the phosphorous chemical industry tail gas,the concentration of which is always more than 80 vol.%,and it can be the feed gas to produce various valuable products such as formate,oxalate,and methanol and so on.But,PH3 is one of the important barriers,which is harmful to the following chemical process.In order to make use of the tail gas,PH3 should be removed firstly,and CO should be covered in the whole purified procedure at the same time.In this work,the modified activated carbon(MAC) was used as the adsorbent to separate PH3 from the mixture tail gas.Series of MAC adsorbents were prepared for the adsorption of PH3,which loaded Cu-Fe and Ce(La),or separately.The PH3 adsorption capacities,chemical and physical properties of MAC were all investigated.The results showed that over 99% PH3 adsorption efficiency was achieved when used MAC adsorbents.The removal efficiency and PH3 adsorption capacity of the Cu-Fe-Ce/AC(20:1:0.4) were both much higher than those modified activated carbons.The maximum PH3 adsorption capacity was 71 mg of PH3/g of MAC on the Cu-Fe-Ce/AC,which were much higher than literature data using CuO only for adsorbing hydride gases.
基金supported by Tianjin University-Qinghai Nationalities University Joint Innovation Fund(no.2016XZC-0034)
文摘In this study, we prepared and applied polymeric porous microsphere adsorbents with selectivity for Li^+ extraction from aqueous solution. We synthesized the adsorbents by suspension polymerization using methacryloyoxyme-12-crown-4(M12C4) as a functional monomer, which had been synthesized from 2-hyroxymethyl-12-crown-4 and methacryloyl chloride. We verified the chemical composition by solid nuclear magnetic resonance(13C-NMR) spectroscopy and observed the porous structure by scanning electron microscopy(SEM). We conducted adsorption isothermal and kinetic tests to determine the adsorption properties. It was found that the adsorbents showed high adsorption efficiency and an adsorption equilibrium time of 200 min. In addition, since the crown ether used in this work could form a stable complex with Li^+, we observed good selectivity for Li^+ in the prepared solution compared with other ions such as Na^+, K^+, Mg^(2+), and Ca^(2+). We reused the adsorbents five times with no significant decrease in adsorptive capacity.
基金Project supported by the National Key Technology Research and Development Program of China(No.2006BAC02A15)Opening Foundation of Jiangsu Provincial Key Laboratory of Coastal Wetland Bioresources and Environmental Protection of China(No.JLCBE05006)the Qinglan Project of Jiangsu Province
文摘The adsorption behavior ofp-aminobenzoic acid and o-aminobenzoic acid onto the different polymeric adsorbents was systematically investigated as a function of the solution concentration and temperature. Experimental results indicated that the equilibrium adsorption data of the four polymeric adsorbents fitted well in the Freundlich isotherm. The adsorption capacity of multi-functional polymeric adsorbent NJ-99 was the highest, which might be attributed to the strong hydrogen-bonding interaction between the amino groups on the resin and the carboxyl group of aminobenzoic acid. The adsorption capacity of o-aminobenzoic acid onto any adsorbent was higher than p-aminobenzoic acid. Thermodynamic studies suggested the exothermic, spontaneous physical adsorption process. Adsorption kinetics results showed that the adsorption followed the pseudo-second-order kinetics model and the intraparticle mass transfer process was the rate-controlling step.
文摘Adsorption equilibrium isotherms of phenolic compounds, phenol, p cresol, p chlorophenol and p nitrophenol, from aqueous solutions by Amberlite XAD 4 polymeric adsorbent and its acetylized derivative MX 4 within temperature range of 283 323K were obtained and fitted to the Freundlich isotherms. The capacities of equilibrium adsorption for all four phenolic compounds from their aqueous solutions increased around 20% on the acetylized resin, which may be contributed to the specific surface area and the partial polarity on the network. Estimations of the isosteric enthalpy, free energy, and entropy for the adsorption process were reported.
基金This project was supported by the National Natural Science Foundation of China (No. 29974015).
文摘This paper presents experimental observations on the adsorption of individual solutes by a simple thermodynamic framework, and the equilibrium adsorption of ethyl benzoate and diethyl phthalate on phenolic resin adsorbent in hexane solutions within the temperature range of 293-313 K. The experimental results show that the Freundlich adsorption law is applicable to the adsorption of ethyl benzoate and diethyl phthalate on the adsorbent, since all the correlative factors R' are larger than 0.99. The negative values of all the isosteric adsorption enthalpies for ethyl benzoate and diethyl phthalate indicate that they undergo exothermic processes, while their magnitudes (19-28 kJ/mol) manifest a hydrogen bonding sorption process. Other thermodynamic properties: the free energy changes and the entropy change associated with the adsorption have been calculated from the Gibbs adsorption equation and the Gibbs-Helmholtz equation
基金supported by the Educational Bureau of Jiangsu Province,China(No.08KJD150020)Jiangsu Provincial Key Laboratory of Coastal Wetland Bio-resources and Environmental Protection(No.JLCBE09011)the Professorial and Doctor Funds of Yancheng Teachers College(No.09YSYJB0202)
文摘Two hypercrosslinked polymeric adsorbents （ZH-01 and Amberlite XAD-4 resin） were employed to remove three kinds of phenolic compounds including phenol, 4-nitrophenol and 2,4-dinitrophenol from aqueous solutions. The study was focused on the static equilibrium adsorption behavior, the column dynamic adsorption and desorption profiles. The Freundlich model gave a perfect fitting to the isotherm data. The adsorbing capacities for these three compounds on ZH-01 were higher than those on Amberlite XAD-4 within the temperature range 288-318 K, which was attributed to the large micropore area and 2-carboxybenzoyl functional groups on the network of ZH-01 resin. The adsorption for phenol and 4- nitrophenol on ZH-01 was a physical adsorption process, while for 2,4-dinitrophenol it was a coexistence process of physical adsorption and chemisorption＇s transitions. The column test showed the advantages of ZH-01 in the dynamic adsorption processes of phenolic compounds. Being used as the desorption reagent, sodium hydroxide solution showed an excellent performance.
基金supported by the National Natural Science Foundation of China (21875107, U1802256, and 22209204)Leading Edge Technology of Jiangsu Province (BK20220009), the Natural Science Foundation of Jiangsu Province (BK20221140)+2 种基金the China Postdoctoral Science Foundation (2022M713364)Jiangsu Specially Appointed Professors ProgramPriority Academic Program Development of Jiangsu Higher Education Institutions (PAPD)。
文摘The solvation structure of Li^(+) in chemical prelithiation reagent plays a key role in improving the low initial Coulombic efficiency(ICE) and poor cycle performance of silicon-based materials. Never theless, the chemical prelithiation agent is difficult to dope active Li^(+) in silicon-based anodes because of their low working voltage and sluggish Li^(+) diffusion rate. By selecting the lithium–arene complex reagent with 4-methylbiphenyl as an anion ligand and 2-methyltetrahydrofuran as a solvent, the as-prepared micro-sized Si O/C anode can achieve an ICE of nearly 100%. Interestingly, the best prelithium efficiency does not correspond to the lowest redox half-potential(E_(1/2)), and the prelithiation efficiency is determined by the specific influencing factors(E_(1/2), Li^(+) concentration, desolvation energy, and ion diffusion path). In addition, molecular dynamics simulations demonstrate that the ideal prelithiation efficiency can be achieved by choosing appropriate anion ligand and solvent to regulate the solvation structure of Li^(+). Furthermore, the positive effect of prelithiation on cycle performance has been verified by using an in-situ electrochemical dilatometry and solid electrolyte interphase film characterizations.
基金The National Natural Science Foundation of China( No. 20274017) and the Nature Science Foundation of Jiangsu Province( No. BK2004415)
文摘The adsorption behaviors of 1-naphthol, 1-naphthylamine and l-naphthol/l-naphthylamine mixtures in water over two macroreticular adsorbents were investigated in single or binary batch systems at 293 K, 303 K and 313 K respectively. All the adsorption isotherms in the studied systems can be adequately fitted by Langmuir model. In the case of aminated macroreticular adsorbent NDA103, 1-naphthol is adsorbed to a larger extent than 1-naphthylamine; while, the opposite trend is found for nonpolar macroreticular adsorbent NDA100. It is noteworthy that at higher temperature（303 K and 313 K）, the total uptake amounts of 1-naphthol and 1-naphthylamine in all binary-component systems are obvious larger than the pure uptake amounts in single-component systems, which is presumably due to the cooperative effect primarily arisen from the hydrogen-bonding interaction between the loaded 1-naphthol and 1-naphthylamine molecules. The simultaneous adsorption systems were confirmed to be helpful to the selective adsorption towards 1-naphthol according to the larger selective index.
基金financial support from the Key Technologies R&D Program of China during the 11th Five-Year Plan period (2006BAD12B03)
文摘In this article, in vitro adsorption of aflatoxin B1 （AFB1） onto different adsorbents was characterized and the result was verified by comparing the growth performance and serum protein levels of broilers exposed to aflatoxin-contamination feed. Main components of adsorbents selected were yeast cell extracts （Product A）, HSCAS （Product B）, and a mixture of yeast product and HSCAS （Product C）, respectively. A total of 240 broilers were assigned to eight treatments, and the effects of three types of adsorbents on growth performance and serum protein levels were evaluated. Results indicated that Product B had the highest in vitro affinity for AFB1, followed by Product C and Product A. Product B bound 97.69% of the AFB1 in solution in 10 min, and it remained over 96.03% in 60 min at pH 8.0. The B-AFB1 complex was much stronger than the other two complexes in vitro condition （P 〈 0.05）. Feed intake （FI） and average daily gain （ADG） decreased （P 〈 0.05） and feed gain ratio increased （P 〈0.05） in the treatment fed aflatoxin-contaminated feed versus treatment on the basal feed. Serum total protein （TP）, albumin （ALB）, and globulin （GLOB） levels were significantly decreased （P〈0.05）. Product B （0.15%） increased growth performance and improved serum protein levels, Product A and Product C were not as effective as Product B. Three adsorbents tested here had sufficient potential to AFBt in some extents and Product B could bind AFB1 more effectively than Product A and Product C. These results indicated that Product B could alleviate some of the AFBt toxic effect in broilers.
基金Supported by the Science and Technology Planning Project of Guangdong(2006A36701004)the Basic Research Program of the Ministry of Environmental Protection(zx_200910_02)
文摘The carbonaceous adsorbent was prepared from mixtures of dewatered sludge and sawdust with enhanced ZnCl2 chemical activation.Characteristics of the adsorbent were studied using scanning electron microscope(SEM) ,Fourier transform infrared spectroscopy(FT-IR) ,and adsorption of nitrogen.The surface analysis showed that the carbonaceous adsorbent had good specific surface and porosity(394 m 2 ·g-1of BET surface,0.12 and 0.10 ml·g-1of microporous and mesoporous volume,respectively) .The oxygen functional groups such as OH,C O and C O were found on the surface by FTIR and XPS(X-ray photoelectron spectroscopy) .The adsorption of elemental mercury(Hg0) on the carbonaceous adsorbent was studied in a fixed bed reactor.The dynamic adsorption capacity of carbonaceous adsorbent increased with influent mercury concentration,from 23.6μg·g-1at 12.58μg·m-3to 87.9μg·g-1at 72.50μg·m-3,and decreased as the adsorption temperature increased,from 246 μg·g-1 at 25°C to 61.3μg·g-1 at 140°C,when dry nitrogen was used as the carrier gas.The carbonaceous adsorbent presented higher dynamic adsorption capacity than activated carbon,which was 81.2μg·g-1and 53.8μg·g-1respectively.The adsorption data were fitted to the Langmuir adsorption model.The physical and chemical adsorption were identified on the adsorbent.
基金Supported by Research Foundation of Overseas Chinese Affairs Office,the State Council,P.R.China,and FujianProvincial Science and Technology Creation Foundation for Young Researchers(No.2 0 0 1J0 2 3)
文摘Sieve effect, complexation, ionic exchange, electrostatic interaction, hydrogen bonding, hydrophobic interaction, and molecular recognition based on molecular imprinting are comprehensively discussed.
基金supported by the National Natural Science Foundation of China(21878200 and 21676174)International S&T Cooperation Program of Shanxi province(201703D421038)+1 种基金Shanxi Scholarship Council of China(2017-036)Joint Fund of Shanxi Provincial Coal Seam Gas(2015012019)。
文摘Global warming and associated global climate change have led to serious efforts towards reducing CO_(2)emissions through the CO_(2)capture from the major emission sources.CO_(2)capture using the amine functionalized adsorbents is regard as a direct and effective way to reducing CO_(2)emissions due to their large CO_(2)adsorption amount,excellent CO_(2)adsorption selectivity and lower energy requirements for adsorbent regeneration.Moreover,large number of achievements on the amine functionalized solid adsorbent have been recorded for the enhanced CO_(2)capture in the past few years.In view of this,we review and analyze the recent advances in amine functionalized solid adsorbents prepared with different supporting materials including mesoporous silica,zeolite,porous carbon materials,metal organic frameworks(MOF)and other composite porous materials.In addition,amine functionalized solid adsorbents derived from waste resources are also reviewed because of the large number demand for cost-effective carbon dioxide adsorbents and the processing needs of waste resources.Considering the importance of the stability of the adsorbent in practical applications,advanced research in the capture cycle stability has also been summarized and analyzed.Finally,we summarize the review and offer the recommendations for the development of amine-based solid adsorbents for carbon dioxide capture.
文摘An ultra-wideband mixing component cascaded by a mixing multi-function chip and a frequency multiplier multi-function chip was demonstrated and implemented using 3D heterogeneous integration based on the silicon adapter board technology.Four layers of high-resistance silicon substrate stack packaging are implemented based on the wafer-level gold-gold bonding process.Each layer adopts though silicon via(TSV)technology to realize signal interconnection.A core monolithic integrated microwave chip(MMIC)is embedded in the silicon cavity,and the silicon-based filter is integrated with the high-resistance silicon substrate.The interconnect line,cavity and filter of the silicon-based adapter board are designed with AutoCAD,and HFSS is adopted for 3D electromagnetic field simulation.According to the measured results,the radio frequency(RF)of the mixing multi-function chip is 40-44 GHz and its intermediate frequency(IF)can cover the Ku band with a chip size of 10 mm×11 mm×1 mm.The multiplier multi-function chip operates at 16-20 GHz.The fundamental suppression is greater than 50 dB and the second harmonic suppression is better than 40 dB with a chip size of 8 mm×8 mm×1 mm.The cascaded fully assembled mixing component achieves a spur of better than-50 dBc and a gain of better than 15 dB.
基金sponsored by the National Science Foundation(CMMI-1562907)the financial support from the National Natural Science Foundation of China(51678511 and 51308484)+4 种基金the Open Fund of Key Laboratory of Mineralogy and Metallogeny in Chinese Academy of Sciences(KLMM20150104)the Natural Science Foundation of Hunan Province(13JJ4049)the Education Department Fund of Hunan Province(14C1094)the Major Talent Training Program of Xiangtan University(16PYZ09)the Specialized Research Fund for the Doctoral Program of Xiangtan University(12QDZ18)
文摘Hybrid adsorbents for COcapture were prepared by coassembling laponite（LP） nanosheets and 1-nbutyl-3-methylimidazolium chloride（BMIMCl）. The prepared BMIMCl/LP layered hybrids were systematically characterized. The interlayer distance of the BMIMCl/LP layered hybrids expanded with an increasing concentration of BMIMCl, indicating that cumulative BMIMCl was intercalated into the LP layers. The efficiency of BMIMCl toward COcapture was significantly enhanced after it was immobilized within LP layers.
